Stability and conductivity of cation- and anion-substituted LiBH4-based solid-state electrolytes

doi:10.1103/PhysRevMaterials.2.065402

CORC > 合肥物质科学研究院 > 中国科学院合肥物质科学研究院 > 中科院固体物理研究所

	Stability and conductivity of cation- and anion-substituted LiBH4-based solid-state electrolytes
	Yao, Zhenpeng 1,2; Kim, Soo 1,3; Michel, Kyle 1,4; Zhang, Yongsheng 1,5; Aykol, Muratahan 1,6; Wolverton, Chris 1
刊名	PHYSICAL REVIEW MATERIALS
	2018-06-19
卷号	2 期号:6 页码:7
ISSN号	2475-9953
DOI	10.1103/PhysRevMaterials.2.065402
通讯作者	Wolverton, Chris(c-wolverton@northwestern.edu)
英文摘要	The high-temperature phase of LiBH4 (HT-LiBH4) exhibits a promisingly high lithium ion conductivity but is unstable at room temperature. We use density functional theory (DFT) calculations to investigate the stabilization effect of halogen and alkali cation/anion substitutions on HT-LiBH4 as well the underlying mechanism for the high lithium ion conductivity. We find that increasing the substituent concentration enhances the stabilization of HT-LiBH4 (i.e., the DFT energy difference between the low- and high-temperature forms of substituted LiBH4 is reduced). Cation/anion substitution also leads to a higher Li defect (vacancy, interstitial, and Frenkel) formation energy, thereby reducing the Li defect (vacancy, interstitial, and Frenkel) concentrations. Using DFT migration barriers input into kinetic Monte Carlo simulations and the Materials INTerface (MINT) framework, we calculate the room-temperature lithium ion conductivities for Li(BH4)(1-x)I-x (x = 0.25 and 0.5) and Li1-yKyBH4 (y = 0.25). Our calculations suggest that the lower I concentration leads to a higher lithium ion conductivity of 5.7 x 10(-3) S /cm compared with that of Li(BH4)(0.5)I-0.5 (4.2 x 10(-5) S/cm) because of the formation of more Lirelated defects. Based on our findings, we suggest that the stabilization of HT-LiBH4-based lithium ion conductors can be controlled by carefully tuning the cation/anion substituent concentrations to maximize the lithium ionic conductivities of the specific system.
资助项目	Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences[DEAC02-06CH11357] ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD)[70NANB14H012] ; US Department of Energy, Office of Science, Basic Energy Sciences[DEFG02-07ER46433] ; Dow Chemical Company ; National Energy Research Scientific Computing Center, a DOE Office of Science User Facility[DE-AC02-05CH11231]
WOS关键词	LITHIUM-ION BATTERIES ; HYDROGEN STORAGE MATERIAL ; MINIMUM ENERGY PATHS ; ELASTIC BAND METHOD ; NANOCONFINED LIBH4 ; RECHARGEABLE BATTERIES ; COMPLEX HYDRIDES ; PHASE-STABILITY ; SADDLE-POINTS ; HIGH-CAPACITY
WOS研究方向	Materials Science
语种	英语
出版者	AMER PHYSICAL SOC
WOS记录号	WOS:000435555100002
资助机构	Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; 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U.S. Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD) ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; US Department of Energy, Office of Science, Basic Energy Sciences ; 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Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; Center for Electrochemical Energy Science (CEES), an Energy Frontier Research Center - US Department of Energy, Office of Science, Basic Energy Sciences ; 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National Energy Research Scientific Computing Center, a DOE Office of Science User Facility ; National Energy Research Scientific Computing Center, a DOE Office of Science User Facility ; National Energy Research Scientific Computing Center, a DOE Office of Science User Facility ; National Energy Research Scientific Computing Center, a DOE Office of Science User Facility
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/37287]
专题	合肥物质科学研究院_中科院固体物理研究所
通讯作者	Wolverton, Chris
作者单位	1.Northwestern Univ, Dept Mat Sci & Engn, 2220 Campus Dr, Evanston, IL 60208 USA 2.Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA 3.MIT, Res Lab Elect, 77 Massachusetts Ave, Cambridge, MA 02139 USA 4.Citrine Informat Inc, 1741 Broadway 300, Redwood City, CA 94063 USA 5.Chinese Acad Sci, Inst Solid State Phys, Key Lab Mat Phys, Hefei 230031, Anhui, Peoples R China 6.Toyota Res Inst, 4440 El Camino Real, Palo Alto, CA 94022 USA
推荐引用方式 GB/T 7714	Yao, Zhenpeng,Kim, Soo,Michel, Kyle,et al. Stability and conductivity of cation- and anion-substituted LiBH4-based solid-state electrolytes[J]. PHYSICAL REVIEW MATERIALS,2018,2(6):7.
APA	Yao, Zhenpeng,Kim, Soo,Michel, Kyle,Zhang, Yongsheng,Aykol, Muratahan,&Wolverton, Chris.(2018).Stability and conductivity of cation- and anion-substituted LiBH4-based solid-state electrolytes.PHYSICAL REVIEW MATERIALS,2(6),7.
MLA	Yao, Zhenpeng,et al."Stability and conductivity of cation- and anion-substituted LiBH4-based solid-state electrolytes".PHYSICAL REVIEW MATERIALS 2.6(2018):7.